High-temperature condensation particle counter

ABSTRACT

Various embodiments include an exemplary design of a high-temperature condensation particle counter (HT-CPC) having particle-counting statistics that are greatly improved over prior art systems since the sample flow of the disclosed HT-CPC is at least eight times greater than the prior art systems. In one embodiment, the HT-CPC includes a saturator block to accept directly a sampled particle-laden gas flow, a condenser block located downstream and in fluid communication with the saturator block, an optics block located downstream and in fluid communication with the condenser block, and a makeup-flow block having a concentric-tube design located in fluid communication with and between the condenser block and the optics block. The makeup-flow block being configured to reduce volatile contents from re-nucleating in the optics block. Other designs and apparatuses are disclosed.

CLAIM OF PRIORITY

This patent application is a U.S. National-Phase Filing under 35 U.S.C.§ 371 from International Application Number PCT/US2019/052113, filed 20Sep. 2019, entitled, “HIGH-TEMPERATURE CONDENSATION PARTICLE,” whichclaims priority to U. S. Provisional. Application Ser. No. 62/734,626,entitled, “HIGH-TEMPERATURE CONDENSATION PARTICLE COUNTER,” filed 21Sep. 2018; the disclosures of which are incorporated herein by referencein their entireties.

TECHNOLOGY FIELD

The disclosed subject matter is generally related to the field ofcounting particles from high-concentration emission sources. Morespecifically, the disclosed subject matter is related to particlecounting and removal of volatile and semi-volatile particles from engineemissions without a need of a volatile particle remover (VPR).

BACKGROUND

A program started within the European Union (EU) entitled the ParticleMeasurement Programme (PMP), sponsored by the Working Group by theUN-ECE GRPE (Working Party on Pollution and Energy), was commissioned todevelop new particle measurement techniques. The PMP focused partiallyon measuring particle emissions at low concentration levels and includedetails of test procedures to be used on, for example, approval testingof light-duty vehicles and heavy-duty engines. A volatile-particleremover (VPR) is currently used by the Particle Measurement Programme toremove volatile and semi-volatile particles from engine emissions. TheVPR, operates at temperatures of up to 400° C. and requires significantquantities of power and filtered dilution air. In addition to the VPR,the specification set by the PMP for a condensation particle counter(CPC) D₅₀ cut-point is 23 nm, to avoid the possibility of themeasurement of volatile artifacts that may occur in some circumstances.

However, it is arguable that the current PMP measurement system has atleast two main drawbacks: (1) the system is complex, expensive, resourcehungry, and bulky; and (2) there may be still be a significant number ofsolid particles below the stated 23 nm cut-point requirement.

Overall, the concept of a high-temperature condensation particle counter(HT-CPC) is to run the CPC at such a high temperature that condensablevapors will stay in vapor form (that is, not counted by the CPC) andhave a much smaller D₅₀ cut-point so that the HT-CPC can measure all orsubstantially all solid particles that are not currently counted by a 23nm cut-point CPC.

Consequently, by having the CPC operating at much higher temperatures,it is possible to achieve the objectives of removing volatile contentswithout the need for the VPR, and the large CPC cut-point (e.g., 23 nmor larger).

FIG. 1 shows a schematic diagram of a high-temperature condensationparticle counter (HT-CPC) 100 of the prior art. The fundamental workingprinciple of the HT-CPC 100 is generally the same as a butanol-basedCPC, known in the art. The main differences are that a different workingfluid is used, and saturator and condenser temperatures are operated atmuch higher temperatures (e.g., greater than 200° C.). The HT-CPC 100includes a saturator block 103, a saturator-flow inlet 105, a poroussilicon-carbide (SiC) diesel particle-filter (DPF) block 109, and acondenser block 113 that is thermally insulated from both an opticalparticle-counter 119 and the saturator block 103 by thermal barriers115, 111, respectively.

With continued reference to FIG. 1, sample air is introduced into anaerosol inlet 101, downstream of the saturator block 103, so that noparticles flow through the saturator block 103. The design of the HT-CPC100 is similar to a TSI® Model 3025 or a TSI® Model 3776 CPC (availablefrom TSI® Incorporated, 500 Cardigan Road, Shoreview, Minn., USA 55126).Nitrogen was used in the original test. The authors of the testsuggested that filtered air could be used as well but no data wereprovided. The SiC DPF block 109 was formed from a silicon-carbide dieselparticle-filter (DPF), which was cut at both ends, thereby rendering theDPF as a through-flow device. The SiC DPF block 109 also functioned as awick for working fluid 107 placed within the saturator block 103.According to the test data, the SiC DPF block 109 wicked well and wasstable at high temperature. The sample flow from the aerosol inlet 101is merged with working-fluid vapor from the saturator block 105 prior toentering the condenser block 113, such that particles were substantiallyconfined around a centerline of the condenser block 113. The condenserblock 113 had a 5 mm outside diameter and was 100 mm in length.

The optical particle-counter 119, comprising a laser 121 and a detector123, used an optics block from a TSI® Model 3034 single-box ScanningMobility Particle Sizer Spectrometer (SNIPS). Two sheath flow inlets 117delivered filtered air orthogonally into the optical particle counter119 to reduce or prevent vapor from condensing and further served tokeep particles from the aerosol inlet 101 from contaminating opticalelements within the optical particle-counter 119. After the particlespass through the optical particle-counter 119, they exit through anoutlet port 125.

The optical particle-counter 119 was run at 45° C., which was much lowerthan temperatures of the condenser block 113. Temperatures in thecondenser block 113 were run at above 200° C. for all working fluids.The working fluids tested comprised perfluorinated polyether (Fomblin® Y6/6 fluid), polyphenyl ether (Santovac® 5), and siloxanes (Dow Corning®DC704 and DC705 silicone-based oil types primarily used for diffusionpumps). However, only the siloxanes were found to achieve a reasonablecounting efficiency.

The information described in this section is provided to offer theskilled artisan a context for the following disclosed subject matter andshould not be considered as admitted prior art.

BRIEF DESCRIPTION OF THE DRAWINGS

FIG. 1 shows a schematic diagram of a high-temperature condensationparticle counter (HT-CPC) of the prior art;

FIG. 2A shows a schematic diagram of an exemplary embodiment of anHT-CPC in accordance with various embodiments disclosed herein;

FIG. 2B shows a schematic diagram of an exemplary embodiment using aclosed-loop design for flow control of the HT-CPC and having two pumps,in accordance with various embodiments disclosed herein;

FIG. 2C shows a schematic diagram of an exemplary embodiment using aclosed-loop design for flow control of the HT-CPC and having a singlepump; in accordance with various embodiments disclosed herein;

FIG. 2D shows a cross-sectional view of an optical chamber of aparticle-counting instrument and an aerosol nozzle having a curtain-flowdevice in accordance with various embodiments of the disclosed subjectmatter;

FIG. 2E shows a cross-sectional view of the optical chamber of theparticle-counting instrument and the aerosol nozzle having acurtain-flow device at Section A-A of FIG. 2D;

FIG. 3 shows a schematic diagram of a tetracontane particle-generatorused to challenge various embodiments of the disclosed HT-CPC units fora volatile-particle test;

FIG. 4A shows a counting-efficiency graph of various embodiments of theHT-CPC disclosed herein, the graph indicates counting efficiency as afunction of particle diameter using sodium-chloride (NaCl) particles totest the HT-CPC;

FIG. 4B shows a graph of particle-counting efficiency as a function ofparticle diameter using sodium chloride particles, classified by adifferential-mobility analyzer (DMA), to challenge various embodimentsof the disclosed HT-CPC; which meets the proposed PMP 10 nm cut pointCPC requirement;

FIG. 4C shows a graph of particle-counting efficiency as a function ofparticle diameter using DMA-classified sodium chloride particles tochallenge various embodiments of the disclosed HT-CPC, which meets thePMP 23 nm cut point CPC requirement;

FIG. 5 shows a counting-efficiency graph of the prior art HT-CPCdiscussed above with reference to FIG. 1 for a variety of differentparticle types;

FIG. 6A shows a linearity graph of various embodiments of the HT-CPCdisclosed herein, the graph indicates normalized counting-efficiency asa function of reference particle concentration;

FIG. 6B shows another linearity graph of various embodiments of theHT-CPC disclosed herein, the graph indicates normalizedcounting-efficiency as a function of reference particle concentration,the range of concentration being greater than the concentration range ofFIG. 6A;

FIG. 7A shows a volatile-particle-test graph for tetracontane particlesdisplayed as an HT-CPC inlet concentration percentage as a function ofaerial concentration (in units of particles per cm³);

FIG. 7B shows a volatile-particle-test graph for tetracontane particlesdisplayed as an HT-CPC inlet concentration percentage as a function ofcondenser temperature for two different HT-CPC units designed inaccordance with the various embodiments disclosed herein; and

FIG. 7C shows a volatile-particle-test graph for Emery oil particlesdisplayed as an HT-CPC inlet concentration percentage as a function ofcondenser temperature for HT-CPC units designed in accordance with thevarious embodiments disclosed herein.

DETAILED DESCRIPTION

The description that follows includes illustrative examples, devices,and apparatuses that embody various aspects of the disclosed subjectmatter. In the following description, for purposes of explanation,numerous specific details are set forth in order to provide anunderstanding of various embodiments of the inventive subject matter. Itwill be evident however, to those of ordinary skill in the art, thatvarious embodiments of the disclosed subject matter may be practicedwithout these specific details. Further, well-known structures,materials, and techniques have not been shown in detail, so as not toobscure the various illustrated embodiments.

As used herein, the term “or” may be construed in an inclusive orexclusive sense. Additionally, although various exemplary embodimentsdiscussed below focus on counting particles from high-concentrationemission sources, the disclosed subject matter is also related toparticle counting and removal of volatile and semi-volatile particlesfrom engine emissions without a need of a volatile particle remover(YPR). Upon reading and understanding the disclosure provided herein, aperson of ordinary skill in the art will readily understand that variouscombinations of the techniques and examples may all be applied seriallyor in various combinations. As an introduction to the subject, a fewembodiments will be described briefly and generally in the followingparagraphs, and then a more detailed description, with reference to thefigures, will ensue.

The various embodiments of the high-temperature condensation particlecounter (HT-CPC) disclosed herein show superior performance overcontemporaneous reported designs, such as the HT-CPC 100 of the priorart as shown and described with reference to FIG. 1. As disclosedherein, the particle-counting statistics of the disclosed embodiments ofthe HT-CPC are greatly improved over prior art systems. For example, thesample flows of the disclosed subject matter are about eight timeshigher than those systems reported previously in the literature.Additionally, the makeup flow and concentric-tube design, discussed inmore detail below, keep the optical elements cool, minimize particlelosses to the nozzle, and prevent or reduce volatile contents fromre-nucleating in the flow path and optics block. The operatingtemperatures of the disclosed subject matter are also lower than thereported, prior art designs and keep the temperatures well below theworking-fluid flash-point of 243° C. (in one exemplary embodiment).Consequently, the lower operating temperatures are advantageous inmaintaining better working-fluid stability and a safer instrument bykeeping the operating temperatures well below flash points of thevarious working-fluids. Further, a working fluid that is chemically morestable allows various ones of the disclosed embodiments of the HT-CPCalso to use air as the carrier gas without having working fluidoxidation and degradation issues, thereby significantly simplifyinginstrument design and reducing the operating cost.

In the following detailed description, reference is made to theaccompanying drawings that form a part of the high-temperature CPC andin which is shown, by way of illustration, specific embodiments. Otherembodiments may be utilized and, for example, various thermodynamic,electrical, or physical changes may be made without departing from thescope of the present disclosure. The following detailed description is,therefore, is to be taken in an illustrative sense rather than in alimiting sense.

In general, a condensation particle counter (also known as acondensation nucleus counter) is used to detect particles in a monitoredenvironment where the particles are too small to scatter enough light tobe detected by conventional detection techniques (e.g., light scatteringof a laser beam in an optical particle counter). The small particles aregrown to a larger size by condensation formed on the particle. That is,each particle serves as a nucleation point for the working fluid. Avapor, which is produced by the working fluid of the particle detectioninstrument, is condensed onto the particles to make them larger. Afterachieving growth of the particle due to condensation of the workingfluid vapor onto the particle, CPCs then function similarly to opticalparticle counters in that the individual droplets subsequently passthrough the focal point (or line) of a laser beam, producing a flash oflight in the form of scattered light. Each light flash is counted as oneparticle. The science of condensation particle counters, and thecomplexity of the instrumentation, lies with the technique to condensevapor onto the particles. When the vapor surrounding the particlesreaches a specific degree of supersaturation, the vapor begins tocondense on the particles. The magnitude of supersaturation determines aminimum-detectable particle size of the CPC. Generally, thesupersaturation profile within the instrument is tightly controlled.

With reference now to FIG. 2A, a schematic diagram of an exemplaryembodiment of an HT-CPC 200 in accordance with various embodimentsdisclosed herein is shown. The HT-CPC 200 is shown to include asaturator block 203, a condenser block 205, a makeup-flow block 215, andan optics block 219. In a specific exemplary embodiment, the opticsblock 219 comprises an optics block from a TSI® Model 3772 CPC having aslightly modified detector board. The modified detector board isconfigured to adjust the particle-counting threshold. However, ingeneral, the optics block 219 incorporates an illumination source (e.g.,a laser) and detection optics similar to or the same as other CPCsdescribed above.

The HT-CPC 200 of FIG. 2A comprises of two flow streams: a sample flowand a makeup flow. Unlike the prior at HT-CPC 100 discussed above withreference to FIG. 1, which incorporates a TSI® Model 3025 CPC-likecapillary flow design, the HT-CPC 200 includes an inlet to allow asampled particle-laden gas flow 201 to be introduced directly into thesaturator block 203. This design has several advantages over the priorart including a higher sample-flow rate (producing a better statisticalsample in less time), a simplified mechanical design, and more accurateand robust flow control and measurement. For example, a sample flow rateof the HT-CPC 200 flow rate is about eight-times greater, or more, thandevices of the prior art. As a result of the higher sample-flow rate,the HT-CPC 200 counting statistics are significantly better than priorart devices.

Further, during operation of the HT-CPC 200, hot gas coming from a flowstream 207 from the condenser block 205 (operating substantially aboveambient temperature as noted below) is merged with a substantiallyparticle-free output gas 214 (at approximately ambient room temperatureof, for example, about 20° C.) providing a makeup gas-flow prior toentering the makeup-flow block 215 and subsequently entering the opticsblock 219. The makeup gas-flow serves at least three purposes: (1)keeping the optics block 219 cool (e.g., to approximately ambient roomtemperature); (2) diluting any excess working fluid vapors andcondensable vapors from the flow stream 207 to reduce or minimize thevapors from re-nucleating within the flow path and in the optics block219; and (3) supplementing the sampled particle-laden gas flow 201 tokeep the optics flow at about, for example, 1 lpm. The concentric designof the makeup-flow block 215 keeps particles from the sampledparticle-laden gas flow 201 confined close to a centerline of the flowpath as the sampled particle-laden gas flow 201 is surrounded by gasfrom the particle-free output gas 214. Consequently, particle losses tonozzles are reduces or minimized in the gas flow 217 entering the opticsblock 219.

The sampled particle-laden gas flow 201 enters the saturator block 203,continues through the condenser block 205, and subsequently enters themakeup-flow block 215 from the flow stream 207. The makeup-flow block215 in this embodiment is an open-loop design. A makeup-flow apparatus209 includes a valve 211, to control a volumetric flow or mass flow ofgas, and a filter 213, to substantially remove any particles from thegas. The filter 213 may comprise various types of particulate-air filterknown in the art, such as a high-efficiency particulate air (HEPA)filter or ultra-low particulate air (ULPA) filter. The valve 211 maycomprise a number of gas-flow control devices known in the art such as aneedle valve, a mass-flow controller, a critical orifice, or other typeof device. An input to the valve 211 may comprise clean, dry air (CDA),nitrogen, or any another gas to provide a substantially particle-freeoutput gas 214 to the makeup-flow block 215.

Except for volumetric flowrates, operating temperatures, and workingfluids, as described in more detail below, the saturator block 203 andthe condenser block 205 function similarly to other types of CPCsdescribed above. An example of a prototype of the HT-CPC 200 wasconstructed using portions of hardware from a TSI® Model 3777 CPC. Toaccommodate the high temperatures encountered by the HT-CPC, O-rings ofthe Model 3777 were replaced with Kalrez® O-rings (available from E. I.DuPont De Nemours and Co., 1007 Market Street, Wilmington, Del. 19898,USA) and Delrin® insulators from the Model 3777 CPC (also available fromE. I. DuPont De Nemours and Co.) were replaced withMacoe-machinable-ceramic pieces (Macor® is available from Corning GlassWorks, Houghton Park, Corning, N.Y. 14830, USA) or otherhigh-temperature insulators.

Unlike conventional CPCs, which typically use thermo-electric devices(TEDs) to control condenser temperatures, various ones of the disclosedembodiments of a temperature of the condenser block 205 of the HT-CPC200 are regulated with, for example, two mica heaters. The saturatorblock 203 also has two mica heaters (although a person of ordinary skillin the art, upon reading and understanding the disclosure providedherein, will recognize that a larger or smaller number, or other typesof heater, may be substituted as well). In this exemplary embodiment,all four heaters are controlled and monitored by standaloneproportional-integral-derivative (PID) controllers. Various saturatorand condenser temperatures were evaluated and the temperatures of thesaturator block 203 and the condenser block 205 were eventually set, inthis exemplary embodiment of the HT-CPC 200, to 235° C. and 160° C.,respectively.

Several workings fluids were evaluated for use in the HT-CPC 200. In aspecific exemplary embodiment, Dow Corning 705 (DC 705), a type ofdiffusion-pump oil, performed for the example conditions disclosedherein. Dow Corning® 705 is a silicone pump-fluid and includespentaphenyl trimethyl trisiloxane. For one embodiment of the HT-CPC 200,a piece of fiberglass insulation was cut and used as a wick. Approximateexemplary operating parameters of the HT-CPC 200 and the HT-CPC 100 ofthe prior art are summarized in Table I, below. Note that thetemperatures for the HT-CPC 200 are lower and well below theworking-fluid flash-point of 243° C. The lower operating temperature maybe advantageous to an increased stability of the working fluid as wellas a safer instrument. Moreover, a working fluid that is chemically morestable allows various ones of the disclosed embodiments of the HT-CPC touse air as the carrier gas without having oxidation and degradationissues of the working fluid, thereby significantly simplifyinginstrument design and reducing operating costs.

TABLE I Operating Parameters HT-CPC 100 HT-CPC 200 (prior art) SampleFlow 0.165 lpm 0.02 lpm Condenser Flow 0.165 lpm 0.275 lpm Optics Flow 1lpm 1 lpm Saturator Temperature 235° C. 290° C. Condenser Temperature160° C. 250° C. Optics Temperature ~24° C. (not 45° C. controlled)Working Fluid DC 705 DC 705 Carrier Gas Air Nitrogen

Referring now to FIG. 2B, a schematic diagram of an exemplary embodimentusing a closed-loop design for flow control of an HT-CPC 230 and havinggas pumps 241, in accordance with various embodiments disclosed herein,is shown. The HT-CPC 230 is shown to include a saturator block 233, acondenser block 235, a makeup-flow block 251, a closed-loopparticle-free gas supply 239, an optics block 253, a downstream filter261, and a downstream critical-orifice 263. The saturator block 233 andthe condenser block 235 may the same as or similar to the saturatorblock 203 and the condenser block 205 of FIG. 2A. However, the saturatorblock 233 and the condenser block 235 of FIG. 2B may be configured tooperate at temperatures dissimilar to those of the saturator block 203and the condenser block 205 of FIG. 2A. Also, the optics block 253 maythe same as or similar to the optics block 219 of FIG. 2A. However, theoptics block 253 of the HT-CPC 230 also incorporates a curtain flowdesign, using a clean, curtain-flow gas 240 from the closed-loopparticle-free gas supply 239. Embodiments of a curtain-flow design aredescribed in more detail with reference to FIGS. 2D and 2E, below.

In an embodiment, the closed-loop particle-free gas supply 239 includesthree sections: a makeup gas-supply section 232, a curtain-flowgas-supply section 234, and a recirculation gas-supply section 236. Asdescribed in more detail below, the gases within these sections use atleast a portion of an outlet flow-stream 242 from the optics block 253to provide an input feed gas to the makeup gas-supply section 232 andthe curtain-flow gas-supply section 234. The makeup gas-supply section232 and the curtain-flow gas-supply section 234 provide substantiallyparticle-free output gas 236 and curtain-flow gas 240.

The makeup gas-supply section 232 includes a gas pump 241, an orifice243 to control a volumetric flow of the gas from the pump, a pressuregauge 245 to monitor a pressure drop across the orifice 243 tofacilitate flow control, a heat exchanger 247, and a filter 249. The gaspumps 241 may comprise one of a variety of gas pumps known in the artsuch as carbon-vane pumps and other rotary pumps, reciprocating pumps,peristaltic pumps, and a variety of other gas-pump types. As is known inthe art, a differential-pressure flow-control device (e.g., a criticalorifice) provides a substantially constant flowrate of a gas undervarying load conditions. With a more capable gas pump, a constantflowrate can also be achieved with choked flow by using a smalleropening orifice. In this case, the orifice 243 is referred to ascritical orifice and the pressure gauge 245 is optional. In order forthe choked flow to function properly, a minimum pressure drop, ΔP, ismaintained across the critical orifice 243 to provide the substantiallyconstant flowrate. Depending on other conditions, the pressure drop intypically maintained in excess of 350 mm Hg (approximately 14 inches ofHg). The optional pressure gauge 245 allows for monitoring the pressuredrop to maintain the substantially constant flowrate. In thisembodiment, the heat exchanger 247 removes heat from the gas to adesired temperature (e.g., approximately ambient room temperature ofapproximately 20° C.). In embodiments, the heat exchanger 247 can alsobe used to add heat to the gas. The filter 249 may be the same as orsimilar to the filter 213 of FIG. 2A. The makeup gas-supply section 232provides clean, filtered gas through the particle-free output gas 238that is fed into the makeup-flow block 251, where the filtered gas iscombined with an outlet flow-stream 237 from the condenser block 235,which includes both the sampled particle-laden gas flow 231 and vaporsfrom working fluid with the saturator block 233, some of which havenucleated onto particles from the sampled particle-laden gas flow 231.An outlet flow-stream 252 includes combined flow-streams from the outletflow-stream 237 and the particle-free output gas 238.

The curtain-flow gas-supply section 234 also includes a gas pump 241, anorifice 243 to control a volumetric flow of the gas from the pump, apressure gauge 245 to monitor a pressure drop across the orifice 243 tofacilitate flow control, a heat exchanger 247, and a filter 249. Each ofthese components within the curtain-flow gas-supply section 234 may bethe same as or similar to the related components of the makeupgas-supply section 232. The curtain-flow gas-supply section 234 providesclean, filtered gas through the curtain-flow gas 240 that is fed intothe optics block 253 to prevent or reduce an amount of particulatematter and vapor contamination on optical elements within the opticsblock 253. As noted above, embodiments of a curtain-flow design aredescribed in more detail with reference to FIGS. 2D and 2E, below.

The recirculation gas-supply section 236 uses at least a portion of theoutlet flow-stream 242 from the optics block 253 to provide an inputfeed gas to the makeup gas-supply section 232 and the curtain-flowgas-supply section 234. The recirculation gas-supply section 236includes a primary filter 255, a secondary filter 257, and a gas dryer259. The primary filter 255 may be the same as or similar to the filter213 of FIG. 2A. The secondary filter 257 may comprise, for example, acharcoal filter. A charcoal filter is known to adsorb certain types ofmolecules such as hydrocarbons and other molecules that may be presentwithin the sampled particle-laden gas flow 231 as well as vapors fromthe working fluid within the saturator block 233. The gas dryer 259 maycomprise, for example, a silica dryer to adsorb at least a portion ofmoisture (e.g., working fluid vapor) from the outlet flow-stream 242.The gas dryer 259 may also comprise one or more other types of chemicalor mechanical dryers (e.g., a compressed-gas dryer) as well.

The downstream filter 261 removes most particles from a remainingportion of an outlet flow-stream from the optics block 253 that are notsent to the recirculation gas-supply section 236. The downstreamcritical-orifice 263 limits an amount of the outlet flow-stream from theoptics block 253 that is released as a clean flow-stream 265 to theenvironment.

Approximate exemplary operating parameters of the HT-CPC 230 aresummarized in Table II, below. Note that the temperatures for the HT-CPC230 are lower and well below the working-fluid flash-point of 243° C.for the Dow Corning® 705 diffusion-pump oil used in this exemplaryembodiment. The lower operating temperature may be advantageous to anincreased stability of the working fluid as well as a safer instrument.A working fluid that is chemically more stable allows the HT-CPC 230 touse air as the carrier gas without having oxidation and degradationissues of the working fluid, thereby significantly simplifyinginstrument design and reducing operating costs.

TABLE II Operating Parameters HT-CPC 230 Operating Parameters SampleFlow 0.2 lpm Condenser Flow 0.2 lpm Optics Flow 2 lpm SaturatorTemperature 230° C. Condenser Temperature 186° C. Optics Temperature~24° C. (not controlled) Working Fluid DC 705 Carrier Gas Air

Referring now to FIG. 2C, a schematic diagram of an exemplary embodimentusing a closed-loop design for flow control of an HT-CPC 270 and havinga single pump, in accordance with various embodiments disclosed hereinis shown. The HT-CPC 270 is similar to the HT-CPC 230 of FIG. 2B.However, rather than having separate sections for the makeup gas-supplysection 232 and the curtain-flow gas-supply section 234, the HT-CPC 270uses a combined makeup and curtain-flow gas-supply section 271 havingthe pump 273, a combined orifice and pressure gauge combination 275, aheat exchanger 277, and a filter 279. Downstream of the filter 279, thegas-supply is split into a particle-free output gas 287 and acurtain-flow gas 289. The curtain-flow gas 289 is controlled by a valve281 and a remaining portion of the gas from the filter 279 is controlledby a differential-pressure flow-control device that comprises an orifice285 and a pressure gauge 283.

The particle-free output gas 287 provides clean, filtered gas through tothe makeup-flow block 251, where the filtered gas is combined with theoutlet flow-stream 237 from the condenser block 235, which includes boththe sampled particle-laden gas flow 231 and vapors from working fluidwith the saturator block 233, some of which have nucleated ontoparticles from the sampled particle-laden gas flow 231. An outletflow-stream 291 from the makeup-flow block 251 includes combinedflow-streams from the outlet flow-stream 237 and the particle-freeoutput gas 287.

The pump 273, the combined orifice and pressure gauge combination 275,the heat exchanger 277, and the filter 279 may be the same as or similarto related components of FIG. 2B. The valve 281 may be the same as orsimilar to the valve 211 of FIG. 2A.

With reference now to FIG. 2D, a cross-sectional view of an opticalchamber 280 of a particle-counting instrument and an aerosol-focusingnozzle 287 having a curtain-flow device in accordance with variousembodiments of the disclosed subject matter are shown. In addition tothe optical chamber 280 and the aerosol-focusing nozzle 287, FIG. 2D isshown to include a pair of collection lenses 283, a condenser lens 297,an aerosol inlet port 281, and an aerosol outlet port 285. As is knownto a person of ordinary skill in the art, the collection lenses 283 andthe condenser lens 297 can take a variety of forms and shapes.

The aerosol-focusing nozzle 287 has an upper portion 293 and an aerosolnozzle outlet 295. In an embodiment, the curtain-flow device comprises aplenum chamber 289A and a curtain-flow concentrating nozzle 289B Duringa particle-counting operation, a combination of the plenum chamber 289Aand the curtain-flow concentrating nozzle 289B provides a clean sheathof airflow, through an open area 291 and over the upper portion 293 ofthe aerosol-focusing nozzle 287.

The plenum chamber 289A and the curtain-flow concentrating nozzle 289Bare formed substantially to be annular or partially annular around theupper portion 293 of the aerosol-focusing nozzle 287. The plenum chamber289A and the curtain-flow concentrating nozzle 289B may therefore beconsidered to have a toroidal shape.

The plenum chamber 289A and the curtain-flow concentrating nozzle 289Bmay be formed from a variety of materials including machined orotherwise formed aluminum, stainless steel, various plastics, and othermachinable or formable materials known in the art. In an embodiment, theplenum chamber 289A and the curtain-flow concentrating nozzle 289B maybe machined or formed from a single piece of material. In anotherembodiment, the plenum chamber 289A and the curtain-flow concentratingnozzle 289B may be machined or formed from two materials, that areeither similar or dissimilar to each other, and that are joined together(e.g., by chemical adhesives, soldering, welding, mechanical fasteners,or other techniques known to a person of ordinary skill in the art).

FIG. 2E shows a cross-sectional view 290 of the optical chamber 280 ofthe particle-counting instrument and the aerosol nozzle having thecurtain-flow device at Section A-A of FIG. 2D. A gas-line connector 292allows gas-line tubing (not shown) to provide a clean (e.g., filtered),curtain gas to a gas-flow inlet 293 to the plenum chamber 289A. In aspecific exemplary embodiment, the gas-line connector 292 is a barbconnector (as shown). However, in other embodiments, the gas-lineconnector 292 may be any type of gas-line connector known in the art(e.g., a Swagelok® tube fitting, available from Swagelok Company, Solon,Ohio, USA). The gas-line tubing may comprise various types of tubingincluding nylon tubing, stainless-steel tubing, brass tubing, or othertypes of tubing known in the art. The clean gas introduced into thegas-flow inlet 293 may comprise air (e.g., clean-dry air (CDA)), aninert gas such as argon or hydrogen, or another type of filtered gasthat is substantially particle free.

With concurrent reference to FIGS. 2D and 2E, during operation of theparticle-counting instrument, a flow of curtain gas enters the opticalchamber 280 through the gas-line connector 292. To ensure the curtaingas enters the optical chamber 280 substantially uniformly, the curtaingas is directed through the plenum chamber 289A and into the opticalchamber 280 through, for example, a narrow opening (e.g., a slit orseries of openings) on an uppermost portion of the curtain-flowconcentrating nozzle 289B. The narrow opening may comprise, for example,a single continuous slit or a series or circular or elongated slits.

One function of the combination of the plenum chamber 289A and thecurtain-flow concentrating nozzle 289B is substantially to equalize flowpressure so that the curtain flow (from the gas-flow inlet 293) can bedistributed substantially evenly around the upper portion 293 of theaerosol-focusing nozzle 287 before passing from the narrow opening inthe curtain-flow concentrating nozzle 289E into the open area 291surrounding the upper portion 293, through the narrow opening.

To enhance flow uniformity further, the curtain flow can also beintroduced tangentially (e.g., at an angle with reference to acircumferential direction of the plenum chamber 289A) into the plenumchamber 289A. When the curtain flow is introduced tangentially, aswirling movement of the flow fills up the plenum chamber 289A andcurtain-flow concentrating nozzle 289B quickly. Once inside the opticalchamber 280, the curtain flow then merges co-axially or nearlyco-axially with the aerosol flow that exits from the aerosol nozzleoutlet 295. Consequently, the aerosol flow is not disrupted and issubstantially uniformly surrounded by the curtain flow. Therefore, allor nearly all of the potential contaminants (e.g., particles and vapors)are contained inside the aerosol flow. The combined aerosol flow andcurtain flow then passes through the focused light-beam, describedabove, where particles are illuminated and counted before exiting fromthe aerosol outlet port 285.

A location of the aerosol outlet port 285 could be anywhere in theoptical chamber 280 as long as it is located downstream of the focusedlight-beam. However, in one embodiment, the location of the aerosoloutlet port 285 is opposite the aerosol-focusing nozzle 287, as shown inFIGS. 2D and 2E. This location provides the shortest distance betweenthe aerosol-focusing nozzle 287 and the aerosol outlet port 285. Whenthe aerosol outlet port 285 is opposite from the aerosol-focusing nozzle287, a probability of contaminants traversing the curtain flow to reachthe sensitive optical components is reduced or minimized. The straightflow path from the aerosol-focusing nozzle 287 to the aerosol outletport 285 also avoids any change in flow direction, which potentiallycould introduce flow disturbances resulting in a higher probability ofparticles and/or working fluid vapors deviating from the flow path andcontaminating the optical chamber 280, including the optical elements(e.g., one or more surfaces of the collection lenses 283 and/or thecondenser lens 297).

In addition to reducing or minimizing contamination within the opticalchamber 280, the curtain flow also provides an added benefit of reducingparticle impaction losses to the walls of the optical chamber 280. Withthe curtain flow, particles are restricted substantially to amiddle-portion of the combined aerosol flow and curtain flow. Forexample, in a CPC instrument, a common issue occurs when warmworking-fluid vapors condense on cooler tubing walls resulting in a“foggy” tubing scenario. If excess condensates are formed, CPC flowrates may be affected, thereby resulting in higher measurementuncertainties. The curtain flow design of the disclosed subject matterhelps to reduce, minimize, or prevent the foggy tubing issue as thecurtain flow allows warm vapors to continue to cool down in themiddle-portion of the flow, while separating warm working-fluid vaporsfrom cool tubing walls.

The co-axial or nearly co-axial curtain flow design of the disclosedsubject matter has many advantages over an orthogonally filteredair-flow design of the prior art. For example, the co-axial or nearlyco-axial curtain flow merges smoothly with the aerosol flow as both flowin the same direction. In comparison, the orthogonally filtered air-flowneeds to turn 90 degrees before merging with the aerosol flow. The90-degree turn in flow direction is likely to generate flow turbulence,which could reduce the effectiveness of the curtain flow. Additionally,to reduce or minimize contamination of the optical chamber 280, theparticle-laden or vapor-laden aerosol flow can be surroundedsubstantially fully and uniformly by the curtain flow.

Counting Efficiency, Linearity, and Volatile-Particle Testing of theVarious Embodiments of the HT-CPC

For the counting-efficiency test to comply with the EU PMP requirementsdescribed above, various embodiments of the HT-CPC units were evaluatedwith differential-mobility-analyzer (DMA)-classified monodisperse,furnace-generated sodium chloride (NaCl) particles. The calibrationreference was a TSL® Model 3068B Aerosol Electrometer. Sample flows fromthe aerosol electrometer were maintained at 1 lpm. For the linearitytesting, DMA-classified 40 nm, atomizer-generated NaCl particles wereused. Various concentration levels of the particles were achieved usinga dilution bridge. For the volatile-particle test, the variousembodiments of the HT-CPC units were challenged with tetracontane.Tetracontane is specified by the PMP and is an isomer of thealiphatic-hydrocarbon family having forty carbon atoms and a chemicalformula of C₄₀H₈₂.

. FIG. 3 shows a schematic diagram of a tetracontane particle-generator300 used to challenge various embodiments of the disclosed HT-CPC unitsfor the volatile-particle test. The tetracontane particle-generator 300is shown to include a heating element 301 (e.g., an electric Bunsen), aflask 303 containing an oil 305 (e.g., corn oil) and a tetracontaneblock 323, a rubber-stopped test tube 307, an oil bath thermocouple 309,a carrier-gas/tetracontane-vapor thermocouple 311, and a carrier-gasinlet tube 313. In operation, the heating element 301 heats the oil 305in the flask 303, which in turn heats the tetracontane block 323. Acarrier gas (e.g., nitrogen or air) is introduced into the carrier-gasinlet tube 313. Vapors of tetracontane are carried into therubber-stopped test tube 307 and are cooled by a cooled quench gasintroduced into a quench-gas inlet tube 315. Because of the quenchingeffect, tetracontane particles are formed by homogeneous nucleation. Thenow-cooled tetracontane-aerosol flow continue to an outlet tube 319 toproduce a tetracontane-aerosol output 321. Excess amounts of thetetracontane aerosol flow not needed for the volatile-particle testingmay be directed to a vent 317.

Referring back now to the use of DMA-classified particles, FIG. 4A showsa counting-efficiency graph 400 of various embodiments of the HT-CPCdisclosed herein; the graph 400 indicates counting efficiency as afunction of particle diameter using sodium-chloride (NaCl) particles totest various embodiments of the HT-CPC. The graph 400 indicates a D₅₀cut-point of approximately 5 nm for the sample HT-CPC unit tested ondifferent days (as indicated by “SAMPLE 1” and “SAMPLE 2”). As furtherindicated by the graph 400, results from the two different days are ingood agreement with each other showing that the performance of theHT-CPC unit is consistent over time. The counting efficiencies for largeparticles (e.g., greater than about 20 nm) are at about 93%. Additionaloptimization of the various embodiments of the HT-CPC units has improvedcounting efficiencies to approximately 100%. At least a portion of theoptimization has been occurred by compensating for diffusion losses.

FIG. 4B shows a graph 410 of particle-counting efficiency as a functionof particle diameter using DMA classified sodium chloride particles tochallenge various embodiments of the disclosed HT-CPC. Theparticle-counting efficiency as a function of particle diameter wasconstructed based on a sampled NaCl gas-flow of 0.2 lpm with a totalflow into the optics block at 2 lpm. A temperature of the saturatorblock was 230° C. and a temperature of the condenser block was 186° C.The counting efficiency at 10 nm is about 69% and consequently readilymeets the newly-proposed PMP 10 nm, CPC cut point requirement whichstating that the counting efficiency at 10 nm needs to be within a rangeof 50% to 70%.

FIG. 4C shows a graph 430 of particle-counting efficiency as a functionof particle diameter using DMA classified sodium chloride particles tochallenge various embodiments of the disclosed. HT-CPC. Theparticle-counting efficiency as a function of particle diameter wasconstructed based on a sampled NaCl gas-flow of 0.2 lpm with a totalflow into the optics block at 2 lpm. A temperature of the saturatorblock was about 200° C. and a temperature of the condenser block wasabout 180° C. The stated operational parameters allow variousembodiments of the disclosed HT-CPC to meet PMP current 23 nm, CPC cutpoint requirement.

In comparison with the counting efficiencies of the various embodimentsof the disclosed HT-CPC, FIG. 5 shows a counting-efficiency graph of theHT-CPC 100 of the prior art, discussed above with reference to FIG. 1,for a variety of different particle types. The particle types includeNaCl particles, dispersed particle gel (DPG) particles, ambientparticles, tetracontane particles, and theoretical counting-efficiencyfor the HT-CPC 100. As is known to a person of ordinary skill in theart, the DPG is a three-phase foam in which DPG particles comprisepolymer particles with viscoelasticity having characteristics of solidparticle. Notice the large error bars in the prior art data of FIG. 5.The large error bars are likely due to uncertainties caused by the smallsample flow rate of the HT-CPC 100 of the prior art, which is about ⅛ orless than the flow rate of the disclosed HT-CPC units.

FIG. 6A shows a linearity graph 600 of various embodiments of the HT-CPCdisclosed herein; the graph 600 indicates normalized counting-efficiencyas a function of reference particle concentration. As indicated, thenormalized counting-efficiency drops by about 4% at 67 K counts/cm³. Thedecrease in concentration is mainly because some of the pulses in thistest dropped below the counting threshold. Therefore, the concentrationlimit can be adjusted to be higher once the low pulse-height thresholdis decreased (as discussed in more detail, below).

FIG. 6B shows another linearity graph 610 of various embodiments of theHT-CPC disclosed herein; the graph 610 indicates normalizedcounting-efficiency as a function of reference particle concentration,the range of concentration being greater (by approximately twice theconcentration) than the concentration range of FIG. 6A

Referring now to FIG. 7A, a volatile-particle-test graph 700 fortetracontane particles displayed as an HT-CPC inlet concentrationpercentage as a function of aerial concentration (in units of particlesper cm³) is shown. Since the tetracontane particle-size distributionsfrom the tetracontane particle-generator 300 of FIG. 3 were fairlynarrow, the tetracontane particles were used in the volatile-particletest without DMA classification. The number of particles detected by theHT-CPC appeared to be a function of tetracontane particle-concentrationat the inlet of the HT-CPC. The HT-CPC particle count increased withincreasing inlet concentration. This increase in measured concentrationmay be due to the volatile contents being re-nucleated when the particleflow was cooled down. The stated PMP volatile-particle protocol of theEU PMP testing described above requires a count of less than 1% of thechallenge particles to be measured. Therefore, the various embodimentsof the HT-CPC disclosed readily meet the PMP stated requirement.

FIG. 7B shows a volatile-particle-test graph 710 for tetracontaneparticles displayed as an HT-CPC inlet concentration percentage as afunction of condenser temperature for two different HT-CPC unitsdesigned in accordance with the various embodiments disclosed herein. Asindicated by the graph 710, the measured HT-CPC/inlet concentrationdecreases with an increasing condenser temperature.

FIG. 7C shows a volatile-particle-test graph 730 for Emery oil particlesdisplayed as an HT-CPC inlet concentration percentage as a function ofcondenser temperature for 1-IT-CPC units designed in accordance with thevarious embodiments disclosed herein. As indicated by the graph 710 ofFIG. 7A, the measured HT-CPC/inlet concentration of the graph 730 alsodecreases for with an increasing condenser temperature.

Overall in constructing the various graphs shown above, the false countrate was about 0.01 counts/cm³ for about 1 hour of measurement. The testresults are summarized in Table III, below.

TABLE III Results Summary Test Results D₅₀ (NaCl) Tunable, from about 5nm to about 23 nm Concentration Limit >67,000 cm⁻³ Volatile Particles<0.71% at 64,000 cm⁻³ False Count 0.01 cm⁻³

CONCLUSIONS

As shown and described herein, various exemplary embodiments of theHT-CPC were developed successfully. The performance of the cariousembodiments meets the D₅₀, concentration limit, and volatile-particlerequirements of the PMP.

The shapes of pulses from light detection of the particles were good andthe pulse heights in even the initial tests were approximately 350 mV.Also, in the initial work using early version of the various embodimentsof the HT-CPC, the counting threshold was set to 200 mV. Noise levelswere acceptable as the false count rate was 0.01 cm⁻³. To increasemargins on the signal-to-noise ratio for production units, pulse heightslarger greater than 500 mV can be used. Results from the various ones ofthe disclosed embodiments of the HT-CPC units suggested that the pulseheights increase with increasing saturator temperature. However, highsaturation temperatures may deplete the working fluid more quickly. Anauto-fill function may be used to replenish the working fluid. Also,without the curtain-flow design described herein, a larger amount ofworking fluid vapors would otherwise condense and deposit on the opticscomponents, thereby requiring more frequent cleaning of the opticalelements.

If needed for extremely high particle concentration measurementconditions, an additional dilution step may be used to lower the inletparticle concentration to reduce or eliminate CPC coincidence errorsand/or vapor depletion. Also, the dilution flow may be heated to ahigher temperature.

Although specific values, ranges of values, and techniques are given forvarious parameters discussed above, these values and techniques areprovided merely to aid the person of ordinary skill in the art inunderstanding certain characteristics of the designs and embodimentsdisclosed herein. Those of ordinary skill in the art will realize, uponreading and understanding the disclosure provided herein, that thesevalues and techniques are presented as examples only and numerous othervalues, ranges of values, techniques, and hardware (including workingfluids) may be employed while still benefiting from the novel designsdiscussed herein that may be employed in various HT-CPC designs.Therefore, the various illustrations of the apparatus are intended toprovide a general understanding of the structure and design of variousembodiments and are not intended to provide a complete description ofall the elements and features of the apparatus that might make use ofthe structures, features, and designs described herein.

Many modifications and variations can be made, as will be apparent, to aperson of ordinary skill in the art upon reading and understanding thedisclosure provided herein. Functionally equivalent methods and deviceswithin the scope of the disclosure, in addition to those enumeratedherein, will be apparent to a person of ordinary skill in the art fromthe foregoing descriptions. Portions and features of some embodimentsmay be included in, or substituted for, those of others. Many otherembodiments will be apparent to those of ordinary skill in the art uponreading and understanding the description provided herein. Suchmodifications and variations are intended to fall within a scope of theappended claims. The present disclosure is therefore to be limited onlyby the terms of the appended claims, along with the full scope ofequivalents to which such claims are entitled. It is also to beunderstood that the terminology used herein is for the purpose ofdescribing particular embodiments only and is not intended to belimiting.

The Abstract of the Disclosure is provided to allow the reader toquickly ascertain the nature of the technical disclosure. The abstractis submitted with the understanding that it will not be used tointerpret or limit the claims. In addition, in the foregoing DetailedDescription, it may be seen that various features may be groupedtogether in a single embodiment for the purpose of streamlining thedisclosure. This method of disclosure is not to be interpreted aslimiting the claims. Thus, the following claims are hereby incorporatedinto the Detailed Description, with each claim standing on its own as aseparate embodiment.

What is claimed is:
 1. A high-temperature condensation particle counter(HT-CPC), comprising: a saturator block configured to accept directly asampled particle-laden gas flow; a condenser block located downstreamand in fluid communication with the saturator block; an optics blocklocated downstream and in fluid communication with the condenser block;a makeup-flow block located in fluid communication with and between thecondenser block and the optics block; and a particle-free gas supplycoupled to the makeup-flow block and configured to supply a makeupgas-flow that is substantially free of particles, the particle-free gassupply comprising at least three sections including a make-up gas-supplysection, a curtain-flow gas-supply section, and a recirculationgas-supply section.
 2. The HT-CPC of claim 1, wherein a temperature ofthe makeup gas-flow is at about ambient room temperature.
 3. The HT-CPCof claim 1, wherein a temperature of the makeup gas-flow is at about atemperature substantially lower than the condenser temperature.
 4. TheHT-CPC of claim 1, wherein the particle-free gas supply is configuredto: keep gases flowing into the optics block below a temperature ofgases leaving the condenser block; dilute excess working fluid vaporsand condensable vapors from the gases leaving the condenser block toreduce the vapors from re-nucleating within the optics block; andsupplement a volumetric flowrate of the sample particle-laden gas flowto maintain an optics gas flowrate at a desired level.
 5. The HT-CPC ofclaim 1, wherein the recirculation gas-supply section is configured toremove excess gas from an output of the optics block to feed gas to themake-up gas-supply section and the curtain-flow gas-supply section. 6.The HT-CPC of claim 1, wherein the make-up flow block comprises aconcentric-tube design.
 7. The HT-CPC of claim 6, wherein theconcentric-tube design of the makeup-flow block is configured to keepsparticles from the sampled particle-laden gas flow near a centerline ofa flow path in the optics block.
 8. A high-temperature condensationparticle counter (HT-CPC), comprising: a saturator block configured toaccept directly a sampled particle-laden gas flow; a condenser blocklocated downstream and in fluid communication with the saturator block;an optics block located downstream and in fluid communication with thecondenser block; a makeup-flow block located in fluid communication withand between the condenser block and the optics block; a particle-freegas supply coupled to the makeup-flow block and configured to supply amakeup gas-flow that is substantially free of particles; and acurtain-flow device in fluid communication with both the particle-freegas supply and the optics block to feed a substantially particle-freegas into the optics block to reduce an amount of particulatecontamination and vapor contamination on optical elements within theoptics block.
 9. The HT-CPC of claim 8, further comprising heaterscoupled to the saturator block and to the condenser block to provideheat to maintain a temperature of the saturator block and the condenserblock of at least about 200° C. and at least about 160° C.,respectively.
 10. The HT-CPC of claim 9, wherein the heaters comprisemica heaters.
 11. The HT-CPC of claim 9, further comprising at least oneproportional-integral-derivative (PID) controller to control theheaters.
 12. The HT-CPC of claim 8, wherein the make-up flow blockcomprises a concentric-tube design.
 13. The HT-CPC of claim 12, whereinthe concentric-tube design of the makeup-flow block is configured tokeeps particles from the sampled particle-laden gas flow near acenterline of a flow path in the optics block.